Broadband dielectric spectroscopy (BDS), differential scanning calorimetry (DSC) and Raman spectroscopy are employed to study a series of nanoscale organic-inorganic hybrid materials (NOHMs) comprising 20 wt% silica nanoparticles and either covalently or ionically-bonded polymer canopies. By comparing the NOHMs to the neat polymers used as canopies in their synthesis, we find that timescales characterizing molecular dynamics in the NOHMs largely depend on the interaction between the inorganic cores and the organic canopies. Interestingly, the NOHM materials retain liquid-like behavior, very much unlike conventional polymer nanocomposites. These findings demonstrate the potential of achieving unique and desired material properties via NOHMs by informed choice of the canopy material.